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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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192 records · Page 11

Photon–photon chemical thermodynamics of frequency conversion processes in highly multimode systems

Abstract Frequency generation in highly multimode nonlinear optical systems is inherently a complex process, giving rise to an exceedingly convoluted landscape of evolution dynamics. While predicting and controlling the global conversion efficiencies in such nonlinear environments has long been considered impossible, here, we formally address this challenge even in scenarios involving a very large number of spatial modes. By utilizing fundamental notions from optical statistical mechanics, we develop a universal theoretical framework that effectively treats all frequency components as chemical reactants/products, capable of undergoing optical thermodynamic reactions facilitated by a variety of multi-wave mixing effects. These photon–photon reactions are governed by conservation laws that directly determine the optical temperatures and chemical potentials of the ensued chemical equilibria for each frequency species. In this context, we develop a comprehensive stoichiometric model and formally derive an expression that relates the chemical potentials to the optical stoichiometric coefficients, in a manner akin to atomic/molecular chemical reactions. This advancement unlocks new predictive capabilities that can facilitate the optimization of frequency generation in highly multimode photonic arrangements, surpassing the limitations of conventional schemes that rely exclusively on nonlinear optical dynamics. Notably, we identify a universal regime of Rayleigh–Jeans thermalization where an optical reaction at near-zero optical temperatures can promote the complete and entropically irreversible conversion of light to the fundamental mode at a target frequency. Our theoretical results are corroborated by numerical simulations in settings where second-harmonic generation, sum-frequency generation and four-wave mixing processes can manifest.

Optics↗

Distinguishing Elements at the Sub‐Nanometer Scale on the Surface of a High Entropy Alloy

Materials in crystalline form possess translational symmetry (TS) when the unit cell is repeated in real space with long- and short-range orders. The periodic potential in the crystal regulates the electron wave function and results in unique band structures, which further define the physical properties of the materials. Amorphous materials lack TS due to the randomization of distances and arrangements between atoms, causing the electron wave function to lack a well-defined momentum. High entropy materials provide another way to break the TS by randomizing the potential strength at periodic atomic sites. The local elemental distribution has a great impact on physical properties in high entropy materials. It is critical to distinguish elements at the sub-nanometer scale to uncover the correlations between the elemental distribution and the material properties. Here, the use of synchrotron X-ray scanning tunneling microscopy (SX-STM) with sub-nm scale resolution in identifying elements on a high entropy alloy (HEA) surface is demonstrated. By examining the elementally sensitive X-ray absorption spectra with an STM tip to enhance the spatial resolution, the elemental distribution on an HEA's surface at a sub-nm scale is extracted. In conclusion, these results open a pathway towards quantitatively understanding high entropy materials and their material properties.

36 MATERIALS SCIENCE↗

High spatial and energy resolution electron energy loss spectroscopy of the magnetic and electric excitations in plasmonic nanorod oligomers

We leverage the high spatial and energy resolution of monochromated aberration-corrected scanning transmission electron microscopy to study the hybridization of cyclic assemblies of plasmonic gold nanorods. Detailed experiments and simulations elucidate the hybridization of the coupled long-axis dipole modes into collective magnetic and electric dipole plasmon resonances. We resolve the magnetic dipole mode in these closed loop oligomers with electron energy loss spectroscopy and confirm the mode assignment with its characteristic spectrum image. The energy splitting of the magnetic mode and antibonding modes increases with the number of polygon edges (n). For the n=3-6 oligomers studied, optical simulations using normal incidence and s-polarized oblique incidence show the respective electric and magnetic modes’ extinction efficiencies are maximized in the n=4 arrangement.

47 OTHER INSTRUMENTATION↗

Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices

Polar vortices in oxide superlattices can be utilized as potential candidates for data storage applications due to their unique polarization topologies. The structure and dipole arrangement in polar vortices has been studied via X-ray scattering techniques, (scanning) transmission electron microscopy ((S)/TEM) and computational calculations. However, the fundamental correlation between the atomic structure and the electronic structure (which is manifested in the chemical bonding) has heretofore not been explored. Further, The hybridization between nominally empty $\textit{d}$ orbitals on the B-site with the occupied O 2$\textit{p}$ orbitals favors the condensation of a polar (ferroelectric) state in $\textit{AB}$O 3 perovskite oxides. The complex, continuously rotating local polarization texture of the vortices, in turn, can result in especially intricate $\textit{d}$- orbital interactions. Soft X-ray spectroscopy can probe these interactions at the transition metal $\textit{L}$-edge, but these techniques do not have the spatial resolution to resolve variations within one vortex (~5 nm region). Electron energy loss spectroscopy (EELS) in the STEM mode uses inelastically scattered electrons to probe the core-shell excitations (empty density of states) of transition metals at atomic resolution.

74 ATOMIC AND MOLECULAR PHYSICS↗

Partial connectomes of labeled dopaminergic circuits reveal non-synaptic communication and axonal remodeling after exposure to cocaine

Dopaminergic (DA) neurons exert profound influences on behavior including addiction. However, how DA axons communicate with target neurons and how those communications change with drug exposure remains poorly understood. We leverage cell type-specific labeling with large volume serial electron microscopy to detail DA connections in the nucleus accumbens (NAc) of the mouse (Mus musculus) before and after exposure to cocaine. We find that individual DA axons contain different varicosity types based on their vesicle contents. Spatially ordering along individual axons further suggests that varicosity types are non-randomly organized. DA axon varicosities rarely make specific synapses (<2%, 6/410), but instead are more likely to form spinule-like structures (15%, 61/410) with neighboring neurons. Days after a brief exposure to cocaine, DA axons were extensively branched relative to controls, formed blind-ended ‘bulbs’ filled with mitochondria, and were surrounded by elaborated glia. Finally, mitochondrial lengths increased by ~2.2 times relative to control only in DA axons and NAc spiny dendrites after cocaine exposure. We conclude that DA axonal transmission is unlikely to be mediated via classical synapses in the NAc and that the major locus of anatomical plasticity of DA circuits after exposure to cocaine are large-scale axonal re-arrangements with correlated changes in mitochondria.

59 BASIC BIOLOGICAL SCIENCES↗

Controlled patterning of crystalline domains by frontal polymerization

Materials with hierarchical architectures that combine soft and hard material domains with coalesced interfaces possess superior properties compared with their homogeneous counterparts. These architectures in synthetic materials have been achieved through deterministic manufacturing strategies such as 3D printing, which require an a priori design and active intervention throughout the process to achieve architectures spanning multiple length scales. Here we harness frontal polymerization spin mode dynamics to autonomously fabricate patterned crystalline domains in poly(cyclooctadiene) with multiscale organization. This rapid, dissipative processing method leads to the formation of amorphous and semi-crystalline domains emerging from the internal interfaces generated between the solid polymer and the propagating cure front. The size, spacing and arrangement of the domains are controlled by the interplay between the reaction kinetics, thermochemistry and boundary conditions. Small perturbations in the fabrication conditions reproducibly lead to remarkable changes in the patterned microstructure and the resulting strength, elastic modulus and toughness of the polymer. Furthermore, this ability to control mechanical properties and performance solely through the initial conditions and the mode of front propagation represents a marked advancement in the design and manufacturing of advanced multiscale materials. Drawing inspiration from biological systems in which structural complexity develops through dissipative reaction–diffusion processes, this study explores a transformative synthetic manufacturing strategy aimed at harnessing the principles underpinning morphogenic growth, unlocking new avenues for advanced materials design and fabrication. Synthetic coupled reaction-transport processes offer a versatile yet relatively underexplored method to manipulate the spatial attributes of synthetic materials10. Here we introduce an innovative manufacturing approach based on frontal ring-opening metathesis polymerization (FROMP) that draws parallels with morphogenic growth and development, enabling the formation of patterned microstructures within polymeric materials.

36 MATERIALS SCIENCE↗

Emergence of spin singlets with inhomogeneous gaps in the kagome lattice Heisenberg antiferromagnets Zn-barlowite and herbertsmithite

The kagome Heisenberg antiferromagnet formed by frustrated spins arranged in a lattice of corner-sharing triangles is a prime candidate for hosting a quantum spin liquid (QSL) ground state consisting of entangled spin singlets. However, the existence of various competing states makes a convincing theoretical prediction of the QSL ground state difficult, calling for experimental clues from model materials. The kagome lattice materials Zn-barlowite (ZnCu 3 (OD) 6 FBr) and herbertsmithite (ZnCu 3 (OD) 6 Cl 2 ) do not exhibit long-range order and are considered the best realizations of the kagome Heisenberg antiferromagnet known so far. In this study, we use 63 Cu nuclear quadrupole resonance combined with the inverse Laplace transform to locally probe the inhomogeneity of delicate quantum ground states affected by disorder. We present direct evidence for the gradual emergence of spin singlets with spatially varying excitation gaps, but even at temperatures far below the super-exchange energy scale their fraction is limited to ~60% of the total spins. Theoretical models need to incorporate the role of disorder to account for the observed inhomogeneously gapped behaviour.

36 MATERIALS SCIENCE↗

Comparison of pyrometry and thermography for thermal analysis of thermite reactions

This article examines the thermal behavior of a laser ignited thermite composed of aluminum and bismuth trioxide. Temperature data were collected during the reaction using a four-color pyrometer and a high-speed color camera modified for thermography. The two diagnostics were arranged to collect data simultaneously, with similar fields of view and with similar data acquisition rates, so that the two techniques could be directly compared. Results show that at initial and final stages of the reaction, a lower signal-to-noise ratio affects the accuracy of the measured temperatures. Both diagnostics captured the same trends in transient thermal behavior, but the average temperatures measured with thermography were about 750 K higher than those from the pyrometer. This difference was attributed to the lower dynamic range of the thermography camera’s image sensor, which was unable to resolve cooler temperatures in the field of view as well as the photomultiplier tube sensors in the pyrometer. Overall, while the camera could not accurately capture the average temperature of a scene, its ability to capture peak temperatures and spatial data make it the preferred method for tracking thermal behavior in thermite reactions.

36 MATERIALS SCIENCE↗

Turbulent flow characteristics in an 84-pin rod bundle for typical and damaged spacer grids

Hexagonal rod bundles arranged in a tightly packed triangular lattice are extensively used for heat transfer and energy generation applications. Staggered spacer grids are used to maintain the structural integrity of gas-cooled fast reactor (GFR) fuel assemblies, while inducing localized turbulence in flow. Damage to these spacer grids results in a disruption of flow fields within these hexagonal fuel bundles. Experimental flow visualizations are critical to identify the differences in local flow properties that the structural damage may cause. This experimental research investigates the flow-field characteristics at a near-wall and center plane in a prototypical 84-pin GFR fuel assembly. Newly installed typical spacers and spacers subject to naturally occurring damage due to material degradation over prolonged experimentation were investigated. Velocity fields were acquired by utilizing the matched-index-of-refraction method to obtain time-resolved particle image velocimetry measurements for a Reynolds number of 12 000. Reynolds decomposition statistical results divulged differences in the time-averaged velocity, velocity fluctuations, flow anisotropy, and Reynolds stress distributions. Galilean decomposition demarcated the influence of spacer grid damage on the velocity fields. To extract turbulent structures and elucidate mechanisms of flow instabilities, proper orthogonal decomposition analysis was employed. Reduced order flow reconstructions enabled the application of vortex identification algorithms to determine the spatial and statistical characteristics of vortices generated. This research work provides unique experimental data on the spacer grid condition-dependent flow. The results offer a deeper understanding of fluid dynamics behavior to support GFR rod bundle design efforts and computational fluid dynamics model validation.

36 MATERIALS SCIENCE↗

Determining protein polarization proteome-wide using physical dissection of individual Stentor coeruleus cells

Cellular components are non-randomly arranged with respect to the shape and polarity of the whole cell. Patterning within cells can extend down to the level of individual proteins and mRNA. But how much of the proteome is actually localized with respect to cell polarity axes? Proteomics combined with cellular fractionation has shown that most proteins localize to one or more organelles but does not tell us how many proteins have a polarized localization with respect to the large-scale polarity axes of the intact cell. Genome-wide localization studies in yeast found that only a few percent of proteins have a localized position relative to the cell polarity axis defined by sites of polarized cell growth. Here, we describe an approach for analyzing protein distribution within a cell with a visibly obvious global patterning - the giant ciliate Stentor coeruleus. Ciliates, including Stentor, have highly polarized cell shapes with visible surface patterning. A Stentor cell is roughly 2mmlong, allowing a ‘‘proteomic dissection’’ in which microsurgery is used to separate cellular fragments along the anterior-posterior axis, followed by comparative proteomic analysis. In our analysis, 25% of the proteome, including signaling proteins, centrin/SFI proteins, and GAS2 orthologs, shows a polarized location along the cell’s anterior-posterior axis. We conclude that a large proportion of all proteins are polarized with respect to global cell polarity axes and that proteomic dissection provides a simple and effective approach for spatial proteomics.

59 BASIC BIOLOGICAL SCIENCES↗

Metaoptics Enabled Multifunctional Imaging

Despite the fact that most microorganisms occupy two- and three-dimensional space in heterogeneous arrangements and in proximity to other microorganisms of different species, much of our current knowledge about their metabolic processes is derived from homogenizing, then analyzing, the chemical content of cultures containing a single microbial species. This project addressed this fundamental dichotomy by developing a set of optical imaging principles combining multiple new technologies. The imaging strategies developed in this project combine metaoptics structures with active in situ nanoscale control of the chemical environment and applied them to a microbial system, Myxococcus xanthus, with particular relevance to the DoE mission. The combination of metaoptical architectures and nanoscale control over the molecular environment enables: (a) precise control over the electromagnetic (EM) field at length scales smaller than the wavelength of light; (b) control of the interaction of the EM field with critical molecular systems in DOE relevant microbes; (c) control over the chemical environment – especially the presence and quantity of reactive oxygen species (ROS) that can affect redox homeostasis; and (d) the ability to ask new kinds of questions not accessible to ‘omics’ approaches or standard methods of biological imaging. These capabilities are applicable to detailed studies of metabolic pathways in microbes and to lignocellulosic biomass deconstruction. To accomplish these objectives, we pursued two over-arching technical goals: (1) the development of new metaoptics-enabled approaches to imaging and spectroscopic characterization; and (2) the development of tools to control the chemical environment of a microbial sample with nanometer-scale precision. Goal 1 was addressed through the design, fabrication, and characterization of new metasurfaces capable of super-resolution imaging through extreme confinement of the optical field. Goal 2 was addressed by controlling the redox potential on the nanoscale in microbial communities and characterizing their effect on intrinsic bacterial fluorophores which act as molecular sentinels and through characterization of soluble factors secreted by Myxococcus xanthus by confocal Raman imaging. The optical imaging/sensing approaches developed here make it possible to use these powerful new imaging and sensing modalities in metabolic studies by making it possible to visualize and track the spatial and temporal expression patterns of natural or engineered pathways in microorganisms.

09 BIOMASS FUELS↗

Development of NDE/NDT Tools for High-Volume & High-Speed Inspection of CFRP Structures in Automotive Manufacturing

Main advantages of the air-coupled ultrasound testing (ACUT) and electromagnetic testing (EMT) techniques for NDE of CFRP composites were non-contact sensing, scalability for high-speed inspection, cost-effectiveness, and non-hazardous operation. Despite these advantages, no systems that would satisfy the project requirements were commercially available. Hence, one of the major efforts of the Michigan State University (MSU) team at the initial stage of the project was to close this technological gap by developing, optimizing, and validating array sensors that would provide sufficient sensitivity, spatial coverage, and resolution for robust defect detection. Optimization of the ACUT and EMT sensor designs was performed using experimentally validated finite element models. Initial experiments using array probes were conducted on relatively flat CFRP samples. In parallel, the MSU team designed and assembled a portable platform with two robotic arms. The robots were equipped with newly designed sensors that enabled high-speed NDE of curved CFRP parts. Presently, the developed robotic platform can be used as a demo/template NDE system, which is easily adaptable to manufacturing environments and in-line NDE. The ACUT NDE system developed by the MSU team used a high-power 4-channel pulser receiver for parallel data acquisition. The array probes were designed by stacking commercially available ACUT transducers, which operated in the frequency range between 100 kHz and 500 kHz. MSU optimized the excitation procedure and developed wave focusing cones so as to reduce the crosstalk between the transducers and to provide higher pulse repletion frequency (PRF). The through-transmission (TT) and single-side access (SSA) inspection modes were successfully implemented. In the TT-ACUT, structural defects in CFRP were detected by passing ultrasonic waves through the test part. Hence, the ACUT transmitters and receivers needed to be placed on the opposite sides of the test part. In the SSA-ACUT, guided waves (GW) were excited in the test part using the transmitters and were sensed by the receivers from the same side. Multi-channel TT-ACUT and SSA-ACUT provided high-speed NDE, and were successfully validated on CFRP test samples with interlaminar delaminations and other embedded defects The EM techniques developed by the MSU team included: 1) eddy current testing (ECT), 2) capacitive imaging (CI) and hybrid dual-mode imaging. In ECT, structural damage was detected in CFRP using coils sensor arrays. In ECT, the excitation magnetic field is generated by passing an alternating current through a coil, which is placed above the test sample. The excitation field penetrates the conductive sample and induces the eddy currents in its transect. In turn, the eddy currents generate the reaction field, which affects the total field sensed by a coil. Hence, the presence of structural flaws will alter the eddy current flow and the picked-up signal. ECT is mostly sensitive to local changes of the electric conductivity of the test sample, and CFRPs are mostly conductive in the direction of carbon fibers. Hence, ECT was well suited for the detection of fiber damage/fiber irregularities. The MSU team developed printed circuit boards (PCB) with coil sensor arrays optimized for NDE of CFRP. Unlike most commercial probes designed for ECT of metallic structures, the MSU array probes were designed for operation in [1-10] MHz frequency range, which was optimal for low-conductive CFRP. Multiple sensing topologies (coil groups excitation/sensing arrangements) were implemented and successfully validated. Capacitive Imaging (CI) technique developed by MSU was complementary to ECT. In contrast to ECT, which was sensitive to local changes of the electrical conductivity, the CI was sensitive to local changes of the dielectric constant. Therefore, CI could provide information about matrix damage/matrix irregularities in CFRP. The MSU CI sensor arrays were made of multiple circular or rectangular open-plate capacitors printed on PCB. Sensors of this type are not commercially available. In addition to ECT and CI, the MSU team developed a hybrid (dual-mode) inductive/capacitive measurement technique that synergistically combined the benefits of inductive and capacitive sensing for rapid NDE of fiber reinforced polymer (FRP) composite structures. Fiber damage and fiber irregularities in FRPs were detected by configuring hybrid sensors as coil sensors. Similarly, matrix damage, matrix irregularities and interlaminar delaminations were detected by configuring hybrid sensors as capacitive sensors. ECT and CI were performed sequentially by means of electronic switching. Hence, eliminating the need for mounting two separate sensor arrays on the probe. Portable robotic platform was developed by MSU for multi-technique high-speed NDE of CFRP test parts. The platform had two 6-axis robots, which enabled inspection of curved parts in approximately a 6×6×6 ft 3 active scan area. On the software side, the MSU team integrated scripts for NDE hardware control with scripts for robot motion control. MSU also implemented automated path planning for the robots, reconstruction of part’s surfaces via stereovision, 3D rendering of inspection data, and image processing algorithms for enhanced defect detection. Automotive composite parts manufactured by Plasan Composites from Phase I were used to validate the ACUT and EMT techniques on representative testbeds. Among those parts were three X-braces for a Dodge Viper, one composite calibration plaque with known defects at known locations, and four other test sections, including sections from a front splitter, a corner section from a composite hood, and a high-pressure RTM panel made using non crimp fabric. Other test samples included CFRP and GFRP calibration plates with fiber/matrix defects fabricated at MSU/CVRC.

36 MATERIALS SCIENCE↗